71 results match your criteria elucidate solution-phase


Enhanced Electrochemical Performance of Aprotic Li-CO Batteries with a Ruthenium-Complex-Based Mobile Catalyst.

Angew Chem Int Ed Engl 2021 Jul 15;60(30):16404-16408. Epub 2021 Jun 15.

Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.

Li-CO batteries are regarded as next-generation high-energy-density electrochemical devices. However, the greatest challenge arises from the formation of the discharge product, Li CO , which would accumulate and deactivate heterogenous catalysts to cause huge polarization. Herein, Ru(bpy) Cl was employed as a solution-phase catalyst for Li-CO batteries and proved to be the most effective one screened so far. Read More

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Non-thermal plasma-induced DMPO-OH yields hydrogen peroxide.

Arch Biochem Biophys 2021 Jul 6;705:108901. Epub 2021 May 6.

Department of Pathology and Biological Responses, Nagoya University Graduate School of Medicine, Showa-Ku, Nagoya, 466-8550, Japan; Center for Low-temperature Plasma Sciences, Nagoya University, Chikusa-ku, Nagoya, 464-8603, Japan. Electronic address:

Recent developments in electronics have enabled the medical applications of non-thermal plasma (NTP), which elicits reactive oxygen species (ROS) and reactive nitrogen species (RNS), such as hydroxyl radical (OH), hydrogen peroxide (HO), singlet oxygen (O), superoxide (O), ozone, and nitric oxide at near-physiological temperatures. In preclinical studies or human clinical trials, NTP promotes blood coagulation, eradication of bacterial, viral and biofilm-related infections, wound healing, and cancer cell death. To elucidate the solution-phase biological effects of NTP in the presence of biocompatible reducing agents, we employed electron paramagnetic resonance (EPR) spectroscopy to quantify OH using a spin-trapping probe, 5,5-dimethyl-1-pyrroline-N-oxide (DMPO); O using a fluorescent probe; and O and HO using luminescent probes in the presence of thiols or tempol. Read More

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Phase Behavior That Enables Solvent-Free Carbonate-Promoted Furoate Carboxylation.

J Phys Chem Lett 2020 Sep 26;11(18):7544-7551. Epub 2020 Aug 26.

Department of Chemistry, Stanford University, Stanford, California 94305, United States.

Solvent-free chemistry has been used to streamline synthesis, reduce waste, and access novel reactivity, but the physical nature of the reaction medium in the absence of solvent is often poorly understood. Here we reveal the phase behavior that enables the solvent-free carboxylation reaction in which carbonate, furan-2-carboxylate (furoate), and CO react to form furan-2,5-dicarboxylate (FDCA). This transformation has no solution-phase analogue and can be applied to convert lignocellulose into performance-advantaged plastics. Read More

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September 2020

Anion Binding Affinity: Acidity versus Conformational Effects.

J Org Chem 2020 06 29;85(12):8074-8084. Epub 2020 May 29.

School of Chemistry, University of New South Wales, Sydney, NSW 2052, Australia.

High-level quantum chemical calculations were used to elucidate the gas- and solution-phase conformational equilibria for a series of symmetrically substituted (thio)ureas, (thio)squaramides, and croconamides. Gas-phase calculations predict that the thermodynamic conformer of many of these anion receptors is not the dual-hydrogen-bond-facilitating anti-anti conformer as is commonly assumed. For ,'-diaryl thiosquaramides and croconamides, the syn-syn conformer is typically the predominant conformer. Read More

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Interface-mediated noble metal deposition on transition metal dichalcogenide nanostructures.

Nat Chem 2020 Mar 24;12(3):284-293. Epub 2020 Feb 24.

Department of Chemistry, The Pennsylvania State University, University Park, PA, USA.

Functionalizing the surfaces of transition metal dichalcogenide (TMD) nanosheets with noble metals is important for electrically contacting them to devices, as well as improving their catalytic and sensing capabilities. Solution-phase deposition provides a scalable approach to the creation of metal-TMD hybrid systems, but controlling such processes remains challenging. Here we elucidate the different pathways by which gold and silver deposit at room temperature onto colloidal 1T-WS, 2H-WS, 2H-MoSe, 2H-WSe, 1T'-MoTe and T-WTe few-layer nanostructures to produce several distinct classes of 0D-2D and 2D-2D metal-TMD hybrids. Read More

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The orientation of a membrane probe from structural analysis by enhanced Raman scattering.

Biochim Biophys Acta Biomembr 2020 02 28;1862(2):183109. Epub 2019 Nov 28.

Department of Physics & Astronomy, Rice University, Houston, TX, United States of America; Department of Chemistry, Rice University, Houston, TX, United States of America. Electronic address:

Small fluorescent molecules are widely used as probes of biomembranes. Different probes optically indicate membrane properties such as the lipid phase, thickness, viscosity, and electrical potential. The detailed molecular mechanisms behind probe signals are not well understood, in part due to the lack of tools to determine probe position and orientation in the membrane. Read More

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February 2020

Nucleation and Growth of Amino Acid and Peptide Supramolecular Polymers through Liquid-Liquid Phase Separation.

Angew Chem Int Ed Engl 2019 12 7;58(50):18116-18123. Epub 2019 Nov 7.

State Key Laboratory of Biochemical Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, P. R. China.

The transition of peptides and proteins from the solution phase into fibrillar structures is a general phenomenon encountered in functional and aberrant biology and is increasingly exploited in soft materials science. However, the fundamental molecular events underpinning the early stages of their assembly and subsequent growth have remained challenging to elucidate. Here, we show that liquid-liquid phase separation into solute-rich and solute-poor phases is a fundamental step leading to the nucleation of supramolecular nanofibrils from molecular building blocks, including peptides and even amphiphilic amino acids. Read More

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December 2019

Drug Solubilization by Means of Partition/Association Equilibrium Using a Modified Nanosized Dendrimeric Biopolymer.

AAPS PharmSciTech 2019 Sep 9;20(7):304. Epub 2019 Sep 9.

Department of Industrial and Physical Pharmacy, Purdue University, 575 Stadium Mall Drive, West Lafayette, Indiana, 47907, USA.

The objective of this study is to elucidate the combined effects of a novel type of material being investigated as a new excipient, an octenylsuccinate-modified dendrimer-like biopolymer (OS-DLB) and poloxamer (PLX), on the solubility of poorly water-soluble compounds. Phenytoin (PHT), griseofulvin (GSF), ibuprofen (IBU), and loratadine (LOR) were used as model compounds. Phase solubility measurements were conducted to determine the relative proportions of API, OS-DLB, and PLX that result in the most stable dendrimeric complexes. Read More

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September 2019

Herringbone-Patterned 3D-Printed Devices as Alternatives to Microfluidics for Reproducible Production of Lipid Polymer Hybrid Nanoparticles.

ACS Omega 2019 Mar 4;4(3):4650-4657. Epub 2019 Mar 4.

San Jose State University, 1 Washington Square, San Jose, California 95112, United States.

Major barriers to the implementation of nanotechnology include reproducible synthesis and scalability. Batch solution phase methods do not appear to have the potential to overcome these barriers. Microfluidic methods have been investigated as a means to enable controllable and reproducible synthesis; however, the most popular constituent of microfluidics, polydimethylsiloxane, is ill-suited for mass production. Read More

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Direct Observation of Redox Mediator-Assisted Solution-Phase Discharging of Li-O Battery by Liquid-Phase Transmission Electron Microscopy.

J Am Chem Soc 2019 May 8;141(20):8047-8052. Epub 2019 May 8.

Center for Nanoparticle Research , Institute for Basic Science , Seoul 08826 , Republic of Korea.

Li-O battery is one of the important next-generation energy storage systems, as it can potentially offer the highest theoretical energy density among battery chemistries reported thus far. However, realization of its high discharge capacity still remains challenging and is hampered by the nature of how the discharge products are formed, causing premature passivation of the air electrode. Redox mediators are exploited to solve this problem, as they can promote the charge transfer from electrodes to the solution phase. Read More

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A Telescoping View of Solute Architectures in a Complex Fluid System.

ACS Cent Sci 2019 Jan 31;5(1):85-96. Epub 2018 Dec 31.

NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6102, United States.

Short- and long-range correlations between solutes in solvents can influence the macroscopic chemistry and physical properties of solutions in ways that are not fully understood. The class of liquids known as complex (structured) fluids-containing multiscale aggregates resulting from weak self-assembly-are especially important in energy-relevant systems employed for a variety of chemical- and biological-based purification, separation, and catalytic processes. In these, solute (mass) transfer across liquid-liquid (water, oil) phase boundaries is the core function. Read More

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January 2019

Spatially Confined Formation and Transformation of Nanocrystals within Nanometer-Sized Reaction Media.

Acc Chem Res 2018 Nov 16;51(11):2867-2879. Epub 2018 Oct 16.

National Creative Research Initiative Center for Nanospace-Confined Chemical Reactions (NCCRs) and Department of Chemistry , Pohang University of Science and Technology (POSTECH) , Pohang 37673 , Korea.

The extensive research performed in the past two decades has enabled the production of a range of colloidal nanocrystals, mostly through solution-based procedures that generate and transform nanostructures in bulk-phase solutions containing precursors and surfactants. However, the understanding and control of each nanocrystal (trans)formation step during the synthesis are still complicated because of the high complexity of this process, in which multiple diverse events such as nucleation, subsequent growth, attachment, and ripening occur simultaneously in bulk suspensions. Unlike well-established solution-based methods, solid-state reactions, which had been at the forefront of traditional inorganic materials chemistry, are quite rarely utilized in the realm of nanomaterials because of the high temperatures required for most solid-state reactions, as a result of which the clusters and NCs are prone to migrate through the bulk reaction medium and sinter together uncontrollably into large particles. Read More

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November 2018

Epitope Mapping by HDX-MS Elucidates the Surface Coverage of Antigens Associated with High Blocking Efficiency of Antibodies to Birch Pollen Allergen.

Anal Chem 2018 10 14;90(19):11315-11323. Epub 2018 Sep 14.

Regeneron Pharmaceuticals , 777 Old Saw Mill River Rd , Tarrytown , New York 10591 , United States.

Epitopes of a native pollen allergen protein, birch Bet v1, against four of the noncompeting anti-Bet v1 antibodies individually or in combination, were identified by solution-phase amide backbone H/D exchange (HDX) coupled with high-resolution Q-TOF or Orbitrap mass spectrometry. The HDX results indicates that the four anti-Bet v1 antibodies protected specific regions of Bet v1, explaining the difference in their blocking efficiency of each antibody against Bet v1 binding to polyclonal IgEs in Bet v1 allergic patients. An in-house HDX-MS system was further developed to explore the surface protection of Bet v1 in the presence of all four antibodies with 100% sequence coverage and high redundancy. Read More

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October 2018

Solution-Phase Conformation and Dynamics of Conjugated Isoindigo-Based Donor-Acceptor Polymer Single Chains.

J Phys Chem Lett 2017 Nov 30;8(22):5479-5486. Epub 2017 Oct 30.

Department of Chemistry, Stanford University , Stanford, California 94305, United States.

Conjugated polymers are the key material in thin-film organic optoelectronic devices due to the versatility of these molecules combined with their semiconducting properties. A molecular-scale understanding of conjugated polymers is important to the optimization of the thin-film morphology. We examine the solution-phase behavior of conjugated isoindigo-based donor-acceptor polymer single chains of various chain lengths using atomistic molecular dynamics simulations. Read More

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November 2017

Comparative Network Analysis of Patients with Non-Small Cell Lung Cancer and Smokers for Representing Potential Therapeutic Targets.

Sci Rep 2017 10 23;7(1):13812. Epub 2017 Oct 23.

Human Antibody Lab, Innovation Center, Pasteur Institute of Iran, Tehran, Iran.

Cigarette smoking is the leading cause of lung cancer worldwide. In this study, we evaluated the serum autoantibody (AAb) repertoires of non-small cell lung cancer (NSCLC) patients and smokers (SM), leading to the identification of overactivated pathways and hubs involved in the pathogenesis of NSCLC. Surface- and solution-phase biopanning were performed on immunoglobulin G purified from the sera of NSCLC and SM groups. Read More

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October 2017

Systematic Analysis of the Relationship among 3D Structure, Bioactivity, and Membrane Permeability of PF1171F, a Cyclic Hexapeptide with Paralyzing Effects on Silkworms.

J Org Chem 2017 11;82(21):11447-11463

Graduate School of Pharmaceutical Sciences, Tohoku University , 6-3 Aza-Aoba, Aramaki, Aoba-ku, Sendai, Miyagi 980-8578, Japan.

PF1171 hexapeptides, a family of cyclic hexapeptides produced by fungi, exhibit paralyzing effects on the larvae of silkworms via oral administration. To elucidate the structural features of PF1171 hexapeptides that are crucial for bioactivity, the relationship among 3D structure, bioactivity, and membrane permeability of PF1171F (the peptide with the highest bioavailability) was systematically analyzed through the synthesis of 22 analogues. The PF1171F analogues were prepared by the solid-phase synthesis of a linear precursor and subsequent solution-phase macrolactamization. Read More

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November 2017

Dispersive Optical Activity of (R)-Methylene Norbornene: Intrinsic Response and Solvation Effects.

J Phys Chem A 2017 Nov 13;121(43):8251-8266. Epub 2017 Oct 13.

Department of Chemistry, Yale University , P.O. Box 208107, New Haven, Connecticut 06520-8107, United States.

The dispersive optical activity of a homoconjugated bicyclic diene, (R)-methylene norbornene (R-MNB), was interrogated under complementary vapor-phase and solution-phase conditions to elucidate the structural/electronic provenance of its unusual chiroptical signatures and to explore the marked influence of environmental perturbations. The intrinsic (isolated-molecule) values of specific rotation measured at 355 and 633 nm (1623.5 ± 5. Read More

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November 2017

A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis.

ACS Cent Sci 2017 May 15;3(5):482-488. Epub 2017 May 15.

Department of Chemistry, University of California, Berkeley, California 94720, United States.

Light driven excitation of gold nanoparticles (GNPs) has emerged as a potential strategy to generate hot carriers for photocatalysis through excitation of localized surface plasmon resonance (LSPR). In contrast, carrier generation through excitation of interband transitions remains a less explored and underestimated pathway for photocatalytic activity. Photoinduced oxidative etching of GNPs with FeCl was investigated as a model reaction in order to elucidate the effects of both types of transitions. Read More

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Unravelling the mechanisms of vibrational relaxation in solution.

Chem Sci 2017 Apr 10;8(4):3062-3069. Epub 2017 Feb 10.

School of Chemistry , University of Bristol , Cantock's Close , Bristol BS8 1TS , UK . Email: ; Email:

We present a systematic study of the mode-specific vibrational relaxation of NO in six weakly-interacting solvents (perfluorohexane, perfluoromethylcyclohexane, perfluorodecalin, carbon tetrachloride, chloroform, and d-chloroform), chosen to elucidate the dominant energy transfer mechanisms in the solution phase. Broadband transient vibrational absorption spectroscopy has allowed us to extract quantum state-resolved relaxation dynamics of the two distinct NO fragments produced from the 340 nm photolysis of NO → NO(X) + NO(A) and their separate paths to thermal equilibrium. Distinct relaxation pathways are observed for the NO bending and stretching modes, even at energies as high as 7000 cm above the potential minimum. Read More

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Predicting Salt Permeability Coefficients in Highly Swollen, Highly Charged Ion Exchange Membranes.

ACS Appl Mater Interfaces 2017 Feb 19;9(4):4044-4056. Epub 2017 Jan 19.

McKetta Department of Chemical Engineering, Center for Energy and Environmental Resources, and Texas Materials Institute, The University of Texas at Austin , 10100 Burnet Road Building 133 (CEER), Austin, Texas 78758, United States.

This study presents a framework for predicting salt permeability coefficients in ion exchange membranes in contact with an aqueous salt solution. The model, based on the solution-diffusion mechanism, was tested using experimental salt permeability data for a series of commercial ion exchange membranes. Equilibrium salt partition coefficients were calculated using a thermodynamic framework (i. Read More

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February 2017

Experimental and Theoretical Investigation of Sodiated Multimers of Steroid Epimers with Ion Mobility-Mass Spectrometry.

J Am Soc Mass Spectrom 2017 Feb 2;28(2):323-331. Epub 2016 Dec 2.

Department of Chemistry, University of Florida, Gainesville, FL, 32611, USA.

Ion mobility-mass spectrometry (IM-MS) has recently seen increased use in the analysis of small molecules, especially in the field of metabolomics, for increased breadth of information and improved separation of isomers. In this study, steroid epimers androsterone and trans-androsterone were analyzed with IM-MS to investigate differences in their relative mobilities. Although sodiated monomers exhibited very similar collision cross-sections (CCS), baseline separation was observed for the sodiated dimer species (R = 1. Read More

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February 2017

In Situ Electron Microscopy Imaging and Quantitative Structural Modulation of Nanoparticle Superlattices.

ACS Nano 2016 11 17;10(11):9801-9808. Epub 2016 Oct 17.

Department of Chemistry, University of California , Berkeley, California 94720, United States.

We use liquid-phase transmission electron microscopy (LP-TEM) to characterize the structure and dynamics of a solution-phase superlattice assembled from gold nanoprisms at the single particle level. The lamellar structure of the superlattice, determined by a balance of interprism interactions, is maintained and resolved under low-dose imaging conditions typically reserved for biomolecular imaging. In this dose range, we capture dynamic structural changes in the superlattice in real time, where contraction and smaller steady-state lattice constants are observed at higher electron dose rates. Read More

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November 2016

Synthesis and Evaluation of 1,8-Disubstituted-Cyclam/Naphthalimide Conjugates as Probes for Metal Ions.

ChemistryOpen 2016 08 3;5(4):375-85. Epub 2016 Aug 3.

School of Chemistry The University of Sydney Sydney NSW 2006 Australia.

Fluorescent molecular probes for metal ions have a raft of potential applications in chemistry and biomedicine. We report the synthesis and photophysical characterisation of 1,8-disubstituted-cyclam/naphthalimide conjugates and their zinc complexes. An efficient synthesis of 1,8-bis-(2-azidoethyl)cyclam has been developed and used to prepare 1,8-disubstituted triazolyl-cyclam systems, in which the pendant group is connected to triazole C4. Read More

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Cryogenic Ion Mobility-Mass Spectrometry: Tracking Ion Structure from Solution to the Gas Phase.

Acc Chem Res 2016 07 23;49(7):1421-8. Epub 2016 Jun 23.

Department of Chemistry, Texas A&M University , College Station, Texas 77843, United States.

Electrospray ionization (ESI) combined with ion mobility-mass spectrometry (IM-MS) is adding new dimensions, that is, structure and dynamics, to the field of biological mass spectrometry. There is increasing evidence that gas-phase ions produced by ESI can closely resemble their solution-phase structures, but correlating these structures can be complicated owing to the number of competing effects contributing to structural preferences, including both inter- and intramolecular interactions. Ions encounter unique hydration environments during the transition from solution to the gas phase that will likely affect their structure(s), but many of these structural changes will go undetected because ESI-IM-MS analysis is typically performed on solvent-free ions. Read More

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Solid State Collapse of a High-Spin Square-Planar Fe(II) Complex, Solution Phase Dynamics, and Electronic Structure Characterization of an Fe(II)2 Dimer.

Inorg Chem 2016 06 16;55(11):5191-200. Epub 2016 May 16.

Department of Chemistry, Center for Catalysis, University of Florida , Gainesville, Florida 32611, United States.

Square-planar high-spin Fe(II) molecular compounds are rare, and until recently, the only four examples of non-macrocyclic or sterically driven molecular compounds of this kind shared a common FeO4 core. The trianionic pincer-type ligand [CF3-ONO]H3 (1) supports the high-spin square-planar Fe(II) complex {[CF3-ONO]FeCl}{Li(Sv)2}2 (2). In the solid state, 2 forms the dimer complex {[CF3-ONO]Fe}2{(μ-Cl)2(μ-LiTHF)4} (3) in 96% yield by simply applying a vacuum or stirring it with pentane for 2 h. Read More

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Sorption of trivalent lanthanides and actinides onto montmorillonite: Macroscopic, thermodynamic and structural evidence for ternary hydroxo and carbonato surface complexes on multiple sorption sites.

Water Res 2016 08 21;99:74-82. Epub 2016 Apr 21.

Paul Scherrer Institute, Laboratory for Waste Management, 5232 Villigen PSI, Switzerland.

The credibility of long-term safety assessments of radioactive waste repositories may be greatly enhanced by a molecular level understanding of the sorption processes onto individual minerals present in the near- and far-fields. In this study we couple macroscopic sorption experiments to surface complexation modelling and spectroscopic investigations, including extended X-ray absorption fine structure (EXAFS) and time-resolved laser fluorescence spectroscopies (TRLFS), to elucidate the uptake mechanism of trivalent lanthanides and actinides (Ln/An(III)) by montmorillonite in the absence and presence of dissolved carbonate. Based on the experimental sorption isotherms for the carbonate-free system, the previously developed 2 site protolysis non electrostatic surface complexation and cation exchange (2SPNE SC/CE) model needed to be complemented with an additional surface complexation reaction onto weak sites. Read More

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When the inhibitor tells more than the substrate: the cyanide-bound state of a carbon monoxide dehydrogenase.

Chem Sci 2016 May 27;7(5):3162-3171. Epub 2016 Jan 27.

Technische Universität Berlin , Institut für Chemie , Sekretariat PC 14 , D-10623 Berlin , Germany . Email: ; Email: ; Email:

Carbon monoxide dehydrogenase (CODH) is a key enzyme for reversible CO interconversion. To elucidate structural and mechanistic details of CO binding at the CODH active site (C-cluster), cyanide is frequently used as an iso-electronic substitute and inhibitor. However, previous studies revealed conflicting results on the structure of the cyanide-bound complex and the mechanism of cyanide-inhibition. Read More

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Salt Bridge Rearrangement (SaBRe) Explains the Dissociation Behavior of Noncovalent Complexes.

J Am Soc Mass Spectrom 2016 06 6;27(6):975-90. Epub 2016 Apr 6.

Department of Biological Chemistry, David Geffen School of Medicine, University of California-Los Angeles, Los Angeles, CA, 90095, USA.

Native electrospray ionization-mass spectrometry, with gas-phase activation and solution compositions that partially release subcomplexes, can elucidate topologies of macromolecular assemblies. That so much complexity can be preserved in gas-phase assemblies is remarkable, although a long-standing conundrum has been the differences between their gas- and solution-phase decompositions. Collision-induced dissociation of multimeric noncovalent complexes typically distributes products asymmetrically (i. Read More

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In situ microscopy of the self-assembly of branched nanocrystals in solution.

Nat Commun 2016 Apr 4;7:11213. Epub 2016 Apr 4.

Department of Nanochemistry, Istituto Italiano di Tecnologia (IIT), via Morego 30, Genova IT-16163, Italy.

Solution-phase self-assembly of nanocrystals into mesoscale structures is a promising strategy for constructing functional materials from nanoscale components. Liquid environments are key to self-assembly since they allow suspended nanocrystals to diffuse and interact freely, but they also complicate experiments. Real-time observations with single-particle resolution could have transformative impact on our understanding of nanocrystal self-assembly. Read More

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Tracking reaction dynamics in solution by pump-probe X-ray absorption spectroscopy and X-ray liquidography (solution scattering).

Chem Commun (Camb) 2016 Mar;52(19):3734-49

Center for Nanomaterials and Chemical Reactions, Institute for Basic Science, Daejeon, 305-701, Republic of Korea. and Department of Chemistry, KAIST, Daejeon 305-701, Republic of Korea.

Characterization of transient molecular structures formed during chemical and biological processes is essential for understanding their mechanisms and functions. Over the last decade, time-resolved X-ray liquidography (TRXL) and time-resolved X-ray absorption spectroscopy (TRXAS) have emerged as powerful techniques for molecular and electronic structural analysis of photoinduced reactions in the solution phase. Both techniques make use of a pump-probe scheme that consists of (1) an optical pump pulse to initiate a photoinduced process and (2) an X-ray probe pulse to monitor changes in the molecular structure as a function of time delay between pump and probe pulses. Read More

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